Selective adsorption using nanoporous materials is an efficient strategy for separating gas mixtures. In a nanoporous material, pores can exist in different shapes and can have different degrees of inter-connectivity. In recent studies, both pore connectivity and tortuosity have been found to affect the adsorption and dynamical properties of ethane and CO2 in silicalite differently. Here, using Monte Carlo simulations, we investigate if these two attributes can affect the selective adsorption of one component from a mixture of ethane and CO2 in silicalite. For this, the adsorption of an equimolar mixture of ethane and CO2 is simulated in 12 models of silicalite—SnZm (n, m = 0, 1, 2, 3 or 4; with n and m denoting, respectively, the fraction (out of 4) of straight and zigzag channels of silicalite that are available for adsorption)—differing in degrees of pore connectivity and tortuosity. The adsorption selectivity in this system is found to exhibit a reversal with the adsorption dominated by ethane at low pressures (below ~1 atm) and by CO2 at higher pressures (above ~10 atm). Pore connectivity is found to suppress the selective adsorption of CO2 at higher pressures and also shifts the selectivity reversal to higher pressures. The selectivity reversal results from a competition between the polarizability-affected adsorption at lower pressures and efficient packing at higher pressures. The efficient packing of CO2 is a compounded effect resulting from the larger effective pore volume available for CO2 due to its stronger interaction with the pore surface and smaller molecular volume. CO2 molecules show a preference to adsorb in non-tortuous pores, and this preference is found to be stronger in the presence of ethane. The effects of pore connectivity and tortuosity elucidated here should be applicable to a wide range of natural and engineered nanoporous materials, and this knowledge could be used to identify materials with better capability for separating and storing CO2 based on their pore attributes.
纳米多孔材料的选择性吸附是分离混合气体的有效方法。在纳米多孔材料中，孔隙可以以不同的形状存在，并且可以具有不同程度的相互连接。近年来的研究发现，孔隙连通性和弯曲度对乙烷和CO2在硅岩中的吸附和动力学性能有不同的影响。在这里，使用蒙特卡罗模拟，我们研究了这两个属性是否会影响乙烷和二氧化碳混合物在硅石中的选择性吸附。为此，在12种硅石- snzm (n, m = 0,1,2,3或4)模型中模拟了乙烷和CO2等摩尔混合物的吸附;其中n和m分别表示可用于吸附的直通道和之字形通道在孔隙连通性和弯曲度上的不同程度的分数。在该体系中，乙烷在低压(低于~ 1atm)和CO2在高压(高于~ 10atm)下的吸附选择性相反。研究发现，孔隙连通性抑制了CO2在高压下的选择性吸附，并将选择性逆转转移到高压下。选择性逆转是由于在较低压力下受极化影响的吸附和在较高压力下的有效填料之间的竞争。CO2的有效填充是CO2与孔表面相互作用更强，有效孔隙体积更大，分子体积更小的复合效应。CO2分子倾向于在非弯曲孔隙中吸附，并且在乙烷存在时这种倾向更强。这里阐明的孔隙连通性和扭曲度的影响应该适用于广泛的天然和工程纳米孔材料，并且这些知识可以用于根据其孔隙属性识别具有更好分离和储存二氧化碳能力的材料。
{"title":"Ethane-CO2 Mixture Adsorption in Silicalite: Influence of Tortuosity and Connectivity of Pores on Selectivity","authors":"S. Gautam, David Cole","doi":"10.3390/c9040116","DOIUrl":"https://doi.org/10.3390/c9040116","url":null,"abstract":"Selective adsorption using nanoporous materials is an efficient strategy for separating gas mixtures. In a nanoporous material, pores can exist in different shapes and can have different degrees of inter-connectivity. In recent studies, both pore connectivity and tortuosity have been found to affect the adsorption and dynamical properties of ethane and CO2 in silicalite differently. Here, using Monte Carlo simulations, we investigate if these two attributes can affect the selective adsorption of one component from a mixture of ethane and CO2 in silicalite. For this, the adsorption of an equimolar mixture of ethane and CO2 is simulated in 12 models of silicalite—SnZm (n, m = 0, 1, 2, 3 or 4; with n and m denoting, respectively, the fraction (out of 4) of straight and zigzag channels of silicalite that are available for adsorption)—differing in degrees of pore connectivity and tortuosity. The adsorption selectivity in this system is found to exhibit a reversal with the adsorption dominated by ethane at low pressures (below ~1 atm) and by CO2 at higher pressures (above ~10 atm). Pore connectivity is found to suppress the selective adsorption of CO2 at higher pressures and also shifts the selectivity reversal to higher pressures. The selectivity reversal results from a competition between the polarizability-affected adsorption at lower pressures and efficient packing at higher pressures. The efficient packing of CO2 is a compounded effect resulting from the larger effective pore volume available for CO2 due to its stronger interaction with the pore surface and smaller molecular volume. CO2 molecules show a preference to adsorb in non-tortuous pores, and this preference is found to be stronger in the presence of ethane. The effects of pore connectivity and tortuosity elucidated here should be applicable to a wide range of natural and engineered nanoporous materials, and this knowledge could be used to identify materials with better capability for separating and storing CO2 based on their pore attributes.","PeriodicalId":9397,"journal":{"name":"C","volume":"17 12","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138603088","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Karthik Rathinam, V. Mauer, C. Bläker, C. Pasel, Lucas Landwehrkamp, D. Bathen, S. Panglisch
Increasing environmental concerns, stricter legal requirements, and a wide range of industrial applications have led to growing demand for activated carbon worldwide. The energy-intensive production of fresh activated carbon causes significant CO2 emissions and contributes to global competition for renewable carbon-based raw materials. Although (thermal) reactivation of spent activated carbon can drastically reduce the demand for fresh material, the reactivation process itself is still mostly based on experience and empirical knowledge locked into activated carbon companies. Despite the vast number of papers published in the field, practically relevant, systematic, and quantitative knowledge on the thermal reactivation process is barely available. This paper presents a simple and robust methodology for the development of a predictive model for the production of reactivated carbon with a defined product quality under energetically optimized conditions. An exhausted activated carbon sample was subjected to 26 reactivation experiments in a specially designed laboratory rotary kiln, whereas the experiments were planned and evaluated with statistical design of experiments. The influence of the reactivation conditions (heating rate, heating time, H2O/N2 volume ratio, and CO2/N2 volume ratio) on the specific surface area, energy consumption, yield, and adsorption capacity for diatrizoic acid were evaluated. The BET surface of the reactivated carbons ranged between 590 m2/g and 769 m2/g, whereas the respective fresh carbon had a BET surface of 843 m2/g. The adsorption capacity for diatrizoic acid measured as the maximum solid phase concentration qm derived from the Langmuir equation varied between 24.4 g/kg and 69.7 g/kg (fresh carbon: 59.6 g/kg). It was possible to describe the dependency of the quality criteria on different reactivation parameters using mathematical expressions, whereas the response surface methodology with nonlinear regression was applied to build the models. A reactivation experiment under statistically optimized conditions resulted in energy savings up to 65%, whereas the properties of the reactivated sample were close to the predicted values.
{"title":"Eliminating Luck and Chance in the Reactivation Process: A Systematic and Quantitative Study of the Thermal Reactivation of Activated Carbons","authors":"Karthik Rathinam, V. Mauer, C. Bläker, C. Pasel, Lucas Landwehrkamp, D. Bathen, S. Panglisch","doi":"10.3390/c9040115","DOIUrl":"https://doi.org/10.3390/c9040115","url":null,"abstract":"Increasing environmental concerns, stricter legal requirements, and a wide range of industrial applications have led to growing demand for activated carbon worldwide. The energy-intensive production of fresh activated carbon causes significant CO2 emissions and contributes to global competition for renewable carbon-based raw materials. Although (thermal) reactivation of spent activated carbon can drastically reduce the demand for fresh material, the reactivation process itself is still mostly based on experience and empirical knowledge locked into activated carbon companies. Despite the vast number of papers published in the field, practically relevant, systematic, and quantitative knowledge on the thermal reactivation process is barely available. This paper presents a simple and robust methodology for the development of a predictive model for the production of reactivated carbon with a defined product quality under energetically optimized conditions. An exhausted activated carbon sample was subjected to 26 reactivation experiments in a specially designed laboratory rotary kiln, whereas the experiments were planned and evaluated with statistical design of experiments. The influence of the reactivation conditions (heating rate, heating time, H2O/N2 volume ratio, and CO2/N2 volume ratio) on the specific surface area, energy consumption, yield, and adsorption capacity for diatrizoic acid were evaluated. The BET surface of the reactivated carbons ranged between 590 m2/g and 769 m2/g, whereas the respective fresh carbon had a BET surface of 843 m2/g. The adsorption capacity for diatrizoic acid measured as the maximum solid phase concentration qm derived from the Langmuir equation varied between 24.4 g/kg and 69.7 g/kg (fresh carbon: 59.6 g/kg). It was possible to describe the dependency of the quality criteria on different reactivation parameters using mathematical expressions, whereas the response surface methodology with nonlinear regression was applied to build the models. A reactivation experiment under statistically optimized conditions resulted in energy savings up to 65%, whereas the properties of the reactivated sample were close to the predicted values.","PeriodicalId":9397,"journal":{"name":"C","volume":"113 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138607627","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sang Jin Kim, Seung-Jae Ha, Jea Uk Lee, Young-Pyo Jeon, Jin-Yong Hong
For high-efficiency and high-stability lithium ion batteries, a silicon oxide-based carbon composite has been developed as an anode material. To minimize structural defects (cracking and pulverization) due to volumetric contraction/expansion during charge/discharge, silicon oxide (SiOx) is adopted. A pitch—a carbon precursor—is introduced to the surface of SiOx using the mechanofusion method. The introduced pitch precursor can be readily transformed into a carbon layer through stabilization and carbonization processes, resulting in SiOx@C. This carbon layer plays a crucial role in buffering the volume expansion of SiOx during lithiation/delithiation processes, enhancing electrical conductivity, and preventing direct contact with the electrolyte. In order to improve the capacity and cycle stability of SiOx, the electrochemical performances of SiOx@C composites are comparatively analyzed according to the mixing ratio of SiOx and pitch, as well as the loading amount in the anode material. Compared to pristine SiOx, the SiOx@C composite prepared through the optimization of the experimental conditions exhibits approximately 1.6 and 1.8 times higher discharge capacity and initial coulombic efficiency, respectively. In addition, it shows excellent capacity retention and cycle stability, even after more than 300 charge and discharge tests.
{"title":"Preparation of Silicon Oxide-Carbon Composite with Tailored Electrochemical Properties for Anode in Lithium-Ion Batteries","authors":"Sang Jin Kim, Seung-Jae Ha, Jea Uk Lee, Young-Pyo Jeon, Jin-Yong Hong","doi":"10.3390/c9040114","DOIUrl":"https://doi.org/10.3390/c9040114","url":null,"abstract":"For high-efficiency and high-stability lithium ion batteries, a silicon oxide-based carbon composite has been developed as an anode material. To minimize structural defects (cracking and pulverization) due to volumetric contraction/expansion during charge/discharge, silicon oxide (SiOx) is adopted. A pitch—a carbon precursor—is introduced to the surface of SiOx using the mechanofusion method. The introduced pitch precursor can be readily transformed into a carbon layer through stabilization and carbonization processes, resulting in SiOx@C. This carbon layer plays a crucial role in buffering the volume expansion of SiOx during lithiation/delithiation processes, enhancing electrical conductivity, and preventing direct contact with the electrolyte. In order to improve the capacity and cycle stability of SiOx, the electrochemical performances of SiOx@C composites are comparatively analyzed according to the mixing ratio of SiOx and pitch, as well as the loading amount in the anode material. Compared to pristine SiOx, the SiOx@C composite prepared through the optimization of the experimental conditions exhibits approximately 1.6 and 1.8 times higher discharge capacity and initial coulombic efficiency, respectively. In addition, it shows excellent capacity retention and cycle stability, even after more than 300 charge and discharge tests.","PeriodicalId":9397,"journal":{"name":"C","volume":" 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138613091","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xiaoyan Wang, Eng Gee Lim, Kai Hoettges, Pengfei Song
Flexible and wearable electronics have attracted significant attention for their potential applications in wearable human health monitoring, care systems, and various industrial sectors. The exploration of wearable strain sensors in diverse application scenarios is a global issue, shaping the future of our intelligent community. However, current state-of-the-art strain sensors still encounter challenges, such as susceptibility to interference under humid conditions and vulnerability to chemical and mechanical fragility. Carbon materials offer a promising solution due to their unique advantages, including excellent electrical conductivity, intrinsic and structural flexibility, lightweight nature, high chemical and thermal stability, ease of chemical functionalization, and potential for mass production. Carbon-based materials, such as carbon nanotubes, graphene, and nanodiamond, have been introduced as strain sensors with mechanical and chemical robustness, as well as water repellency functionality. This review reviewed the ability of carbon nanotubes-, graphene-, and nanodiamond-based strain sensors to withstand extreme conditions, their sensitivity, durability, response time, and diverse applications, including strain/pressure sensors, temperature/humidity sensors, and power devices. The discussion highlights the promising features and potential advantages offered by these carbon materials in strain sensing applications. Additionally, this review outlines the existing challenges in the field and identifies future opportunities for further advancement and innovation.
{"title":"A Review of Carbon Nanotubes, Graphene and Nanodiamond Based Strain Sensor in Harsh Environments","authors":"Xiaoyan Wang, Eng Gee Lim, Kai Hoettges, Pengfei Song","doi":"10.3390/c9040108","DOIUrl":"https://doi.org/10.3390/c9040108","url":null,"abstract":"Flexible and wearable electronics have attracted significant attention for their potential applications in wearable human health monitoring, care systems, and various industrial sectors. The exploration of wearable strain sensors in diverse application scenarios is a global issue, shaping the future of our intelligent community. However, current state-of-the-art strain sensors still encounter challenges, such as susceptibility to interference under humid conditions and vulnerability to chemical and mechanical fragility. Carbon materials offer a promising solution due to their unique advantages, including excellent electrical conductivity, intrinsic and structural flexibility, lightweight nature, high chemical and thermal stability, ease of chemical functionalization, and potential for mass production. Carbon-based materials, such as carbon nanotubes, graphene, and nanodiamond, have been introduced as strain sensors with mechanical and chemical robustness, as well as water repellency functionality. This review reviewed the ability of carbon nanotubes-, graphene-, and nanodiamond-based strain sensors to withstand extreme conditions, their sensitivity, durability, response time, and diverse applications, including strain/pressure sensors, temperature/humidity sensors, and power devices. The discussion highlights the promising features and potential advantages offered by these carbon materials in strain sensing applications. Additionally, this review outlines the existing challenges in the field and identifies future opportunities for further advancement and innovation.","PeriodicalId":9397,"journal":{"name":"C","volume":"2 6","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"134992039","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chhabi Lal Gnawali, Lok Kumar Shrestha, Jonathan P. Hill, Renzhi Ma, Katsuhiko Ariga, Mandira Pradhananga Adhikari, Rinita Rajbhandari, Bhadra P. Pokharel
High-surface-area porous carbon materials with high porosity and well-defined pore structures are the preferred advanced supercapacitors electrode materials. Here, we report the electrochemical supercapacitive performance of novel high-porosity activated carbon materials prepared from biowaste Terminalia chebula (Harro) seed stones involving zinc chloride (ZnCl2) activation. Activation is achieved by mixing ZnCl2 with Harro seed powder (1:1 w/w) followed by carbonization at 400–700 °C under a nitrogen gas atmosphere. The amorphous carbon materials obtained exhibit excellent performance as electrical double-layer capacitor electrodes in aqueous electrolyte (1 M sulfuric acid) due to high specific surface areas (as high as 1382.6 m2 g−1) based on well-developed micropore and mesopore structures, and partial graphitic structure containing oxygenated surface functional groups. An electrode prepared using material having the optimal surface textural properties achieved a large specific capacitance of 328.6 F g−1 at 1 A g−1 in a three-electrode cell setup. The electrode achieved a good capacitance retention of 44.7% at a high 50 A g−1 current density and outstanding cycling performance of 98.2% even following 10,000 successive charge/discharge cycles. Electrochemical data indicate the significant potential of Terminalia chebula seed-derived porous carbons as high-performance electrode materials for high-energy-storage supercapacitor applications.
具有高孔隙率和良好孔隙结构的高表面积多孔碳材料是先进超级电容器电极材料的首选。本文报道了一种新型的高孔隙度活性炭材料的电化学超电容性能，该材料是由生物废弃物Terminalia chebula (Harro)种子石制备的，涉及氯化锌(ZnCl2)活化。活化是通过将ZnCl2与哈罗籽粉(1:1 w/w)混合，然后在氮气气氛下在400-700℃下碳化来实现的。所制得的非晶态碳材料具有高比表面积(高达1382.6 m2 g−1)，具有良好的微孔和介孔结构，以及含有氧化表面官能团的部分石墨结构，在水电解质(1m硫酸)中具有优异的双电层电容器电极性能。使用具有最佳表面纹理特性的材料制备的电极在三电极电池装置中在1ag−1下获得了328.6 F g−1的大比电容。在50 a g−1电流密度下，该电极的电容保持率为44.7%，即使在10,000次连续充放电循环后，其循环性能也达到98.2%。电化学数据表明，慈兰种子衍生的多孔碳作为高性能储能超级电容器电极材料具有巨大的潜力。
{"title":"Nanoporous Activated Carbon Material from Terminalia chebula Seed for Supercapacitor Application","authors":"Chhabi Lal Gnawali, Lok Kumar Shrestha, Jonathan P. Hill, Renzhi Ma, Katsuhiko Ariga, Mandira Pradhananga Adhikari, Rinita Rajbhandari, Bhadra P. Pokharel","doi":"10.3390/c9040109","DOIUrl":"https://doi.org/10.3390/c9040109","url":null,"abstract":"High-surface-area porous carbon materials with high porosity and well-defined pore structures are the preferred advanced supercapacitors electrode materials. Here, we report the electrochemical supercapacitive performance of novel high-porosity activated carbon materials prepared from biowaste Terminalia chebula (Harro) seed stones involving zinc chloride (ZnCl2) activation. Activation is achieved by mixing ZnCl2 with Harro seed powder (1:1 w/w) followed by carbonization at 400–700 °C under a nitrogen gas atmosphere. The amorphous carbon materials obtained exhibit excellent performance as electrical double-layer capacitor electrodes in aqueous electrolyte (1 M sulfuric acid) due to high specific surface areas (as high as 1382.6 m2 g−1) based on well-developed micropore and mesopore structures, and partial graphitic structure containing oxygenated surface functional groups. An electrode prepared using material having the optimal surface textural properties achieved a large specific capacitance of 328.6 F g−1 at 1 A g−1 in a three-electrode cell setup. The electrode achieved a good capacitance retention of 44.7% at a high 50 A g−1 current density and outstanding cycling performance of 98.2% even following 10,000 successive charge/discharge cycles. Electrochemical data indicate the significant potential of Terminalia chebula seed-derived porous carbons as high-performance electrode materials for high-energy-storage supercapacitor applications.","PeriodicalId":9397,"journal":{"name":"C","volume":"55 10","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"134991876","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
As heterogeneous catalysis is a practical method for activating Oxone, the immobilization of transition metals (e.g., Co, Fe) on carbonaceous supports is a promising platform. Thus, this study attempts to develop a carbon-supported metallic catalyst by growing Co/Fe on carbon foam (CF) via adopting melamine foam as a readily available template which could be transferred to nitrogen-doped CF with marcoporous structures. Specifically, a unique adornment of Co/Fe species on this CF is facilely fabricated through a complexation of Co/Fe with a plant extract, tannic acid, on melamine foam, followed by carbonization to produce nano-needle-like Co/Fe on N-doped CF, forming a magnetic CF (MCF). This resultant MCF exhibits a much higher surface area of 54.6 m2/g than CF (9.5 m2/g), and possesses a much larger specific capacitance of 9.7 F/g, than that of CF as 4.0 F/g. These superior features of MCF enable it to accelerate Oxone activation in order to degrade an emerging contaminant, bis(4-hydroxyphenyl)methanone (BHPM). Furthermore, MCF + Oxone exhibits a lower activation energy as 18.6 kJ/mol for BHPM elimination and retains its effectiveness in eliminating BHPM over multiple rounds. More importantly, the CF is also prepared and directly compared with the MCF to study the composition-structure-property relationship to provide valuable insights for further understanding of catalytic behaviors, surficial characteristics, and application of such a functional carbon material.
{"title":"Magnetic Carbon Foam Adorned with Co/Fe Nanoneedles as an Efficient Activator of Oxone for Oxidative Environmental Remediation: Roles of Surficial and Chemical Enhancement","authors":"Yi-Chun Chen, Xin-Yu Jiang, Bui Xuan Thanh, Jia-Yin Lin, Haitao Wang, Chao-Wei Huang, Hongta Yang, Afshin Ebrahimi, Sanya Sirivithayapakorn, Kun-Yi (Andrew) Lin","doi":"10.3390/c9040107","DOIUrl":"https://doi.org/10.3390/c9040107","url":null,"abstract":"As heterogeneous catalysis is a practical method for activating Oxone, the immobilization of transition metals (e.g., Co, Fe) on carbonaceous supports is a promising platform. Thus, this study attempts to develop a carbon-supported metallic catalyst by growing Co/Fe on carbon foam (CF) via adopting melamine foam as a readily available template which could be transferred to nitrogen-doped CF with marcoporous structures. Specifically, a unique adornment of Co/Fe species on this CF is facilely fabricated through a complexation of Co/Fe with a plant extract, tannic acid, on melamine foam, followed by carbonization to produce nano-needle-like Co/Fe on N-doped CF, forming a magnetic CF (MCF). This resultant MCF exhibits a much higher surface area of 54.6 m2/g than CF (9.5 m2/g), and possesses a much larger specific capacitance of 9.7 F/g, than that of CF as 4.0 F/g. These superior features of MCF enable it to accelerate Oxone activation in order to degrade an emerging contaminant, bis(4-hydroxyphenyl)methanone (BHPM). Furthermore, MCF + Oxone exhibits a lower activation energy as 18.6 kJ/mol for BHPM elimination and retains its effectiveness in eliminating BHPM over multiple rounds. More importantly, the CF is also prepared and directly compared with the MCF to study the composition-structure-property relationship to provide valuable insights for further understanding of catalytic behaviors, surficial characteristics, and application of such a functional carbon material.","PeriodicalId":9397,"journal":{"name":"C","volume":"65 4","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136283476","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Christoph W. Thurner, Leander Haug, Daniel Winkler, Christoph Griesser, Matthias Leitner, Toni Moser, Daniel Werner, Marco Thaler, Lucas A. Scheibel, Thomas Götsch, Emilia Carbonio, Julia Kunze-Liebhäuser, Engelbert Portenkirchner, Simon Penner, Bernhard Klötzer
For the direct reduction of CO2 and H2O in solid oxide electrolysis cells (SOECs) with cermet electrodes toward methane, a fundamental understanding of the role of elemental carbon as a key intermediate within the reaction pathway is of eminent interest. The present synchrotron-based in situ near-ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS) study shows that alloying of Ni/yttria-stabilized-zirconia (YSZ) cermet electrodes with Cu can be used to control the electrochemical accumulation of interfacial carbon and to optimize its reactivity toward CO2. In the presence of syngas, sufficiently high cathodic potentials induce excess methane on the studied Ni/yttria-stabilized-zirconia (YSZ)-, NiCu/YSZ- and Pt/gadolinium-doped-ceria (GDC) cermet systems. The hydrogenation of carbon, resulting from CO activation at the triple-phase boundary of Pt/GDC, is most efficient.
{"title":"Electrocatalytic Enhancement of CO Methanation at the Metal–Electrolyte Interface Studied Using In Situ X-ray Photoelectron Spectroscopy","authors":"Christoph W. Thurner, Leander Haug, Daniel Winkler, Christoph Griesser, Matthias Leitner, Toni Moser, Daniel Werner, Marco Thaler, Lucas A. Scheibel, Thomas Götsch, Emilia Carbonio, Julia Kunze-Liebhäuser, Engelbert Portenkirchner, Simon Penner, Bernhard Klötzer","doi":"10.3390/c9040106","DOIUrl":"https://doi.org/10.3390/c9040106","url":null,"abstract":"For the direct reduction of CO2 and H2O in solid oxide electrolysis cells (SOECs) with cermet electrodes toward methane, a fundamental understanding of the role of elemental carbon as a key intermediate within the reaction pathway is of eminent interest. The present synchrotron-based in situ near-ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS) study shows that alloying of Ni/yttria-stabilized-zirconia (YSZ) cermet electrodes with Cu can be used to control the electrochemical accumulation of interfacial carbon and to optimize its reactivity toward CO2. In the presence of syngas, sufficiently high cathodic potentials induce excess methane on the studied Ni/yttria-stabilized-zirconia (YSZ)-, NiCu/YSZ- and Pt/gadolinium-doped-ceria (GDC) cermet systems. The hydrogenation of carbon, resulting from CO activation at the triple-phase boundary of Pt/GDC, is most efficient.","PeriodicalId":9397,"journal":{"name":"C","volume":"7 6","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135391877","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nemanja Gavrilov, Stefan Breitenbach, Christoph Unterweger, Christian Fürst, Igor A. Pašti
Understanding the properties and behavior of carbon materials is of paramount importance in the pursuit of sustainable energy solutions and technological advancements. As versatile and abundant resources, carbon materials play a central role in various energy conversion and storage applications, making them essential components in the transition toward a greener and more efficient future. This study explores the impact of diammonium hydrogen phosphate (DAHP) impregnation on activated carbon fibers (ACFs) for efficient energy storage and conversion applications. The viscose fibers were impregnated with varying DAHP concentrations, followed by carbonization and activation processes. The capacitance measurements were conducted in 6 mol dm−3 KOH, 0.5 mol dm−3 H2SO4, and 2 mol dm−3 KNO3 solutions, while the oxygen reduction reaction (ORR) measurements were performed in O2-saturated 0.1 mol dm−3 KOH solution. We find that the presented materials display specific capacitances up to 160 F g−1 when the DAHP concentration is in the range of 1.0 to 2.5%. Moreover, for the samples with lower DAHP concentrations, highly selective O2 reduction to peroxide was achieved while maintaining low ORR onset potentials. Thus, by impregnating viscose fibers with DAHP, it is possible to tune their electrochemical properties while increasing the yield, enabling the more sustainable and energy-efficient synthesis of advanced materials for energy conversion applications.
{"title":"Exploring the Impact of DAHP Impregnation on Activated Carbon Fibers for Efficient Charge Storage and Selective O2 Reduction to Peroxide","authors":"Nemanja Gavrilov, Stefan Breitenbach, Christoph Unterweger, Christian Fürst, Igor A. Pašti","doi":"10.3390/c9040105","DOIUrl":"https://doi.org/10.3390/c9040105","url":null,"abstract":"Understanding the properties and behavior of carbon materials is of paramount importance in the pursuit of sustainable energy solutions and technological advancements. As versatile and abundant resources, carbon materials play a central role in various energy conversion and storage applications, making them essential components in the transition toward a greener and more efficient future. This study explores the impact of diammonium hydrogen phosphate (DAHP) impregnation on activated carbon fibers (ACFs) for efficient energy storage and conversion applications. The viscose fibers were impregnated with varying DAHP concentrations, followed by carbonization and activation processes. The capacitance measurements were conducted in 6 mol dm−3 KOH, 0.5 mol dm−3 H2SO4, and 2 mol dm−3 KNO3 solutions, while the oxygen reduction reaction (ORR) measurements were performed in O2-saturated 0.1 mol dm−3 KOH solution. We find that the presented materials display specific capacitances up to 160 F g−1 when the DAHP concentration is in the range of 1.0 to 2.5%. Moreover, for the samples with lower DAHP concentrations, highly selective O2 reduction to peroxide was achieved while maintaining low ORR onset potentials. Thus, by impregnating viscose fibers with DAHP, it is possible to tune their electrochemical properties while increasing the yield, enabling the more sustainable and energy-efficient synthesis of advanced materials for energy conversion applications.","PeriodicalId":9397,"journal":{"name":"C","volume":"39 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135634251","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nina K. Plugotarenko, Sergey P. Novikov, Tatiana N. Myasoedova, Tatiana S. Mikhailova
The low selectivity of materials to gases of a similar nature may limit their use as sensors. Knowledge of the adsorption kinetic characteristics of each gas on the surface of the material may enable the ability to identify them. In this work, copper-containing silicon–carbon films were formed using electrochemical deposition on the Al2O3 substrate with interdigitated Cr/Cu/Cr electrodes. These films showed good adsorption characteristics with several different gases. The adsorption kinetics of nitrogen dioxide, sulfur dioxide, and carbon monoxide on the film surface were investigated by the change in the resistivity of the material. Pseudo-first-order and pseudo-second-order kinetics, Elovich, Ritchie, and Webber intraparticle diffusion models were applied. It was found that the largest approximation factor and the lowest Root-Mean-Square Error and Mean Bias Error for all three gases were for the Elovich model. The advantages of silicon–carbon copper-containing films for gas sensor applications were shown. An algorithm for gas recognition was proposed based on the dependence of the change in the resistivity of the material under stepwise gas exposure. It was found that parameters such as the values of the extrema of the first and second derivatives of the R vs. t dependence during adsorption and the slope of R vs. t dependence in the Elovich coordinates are responsible for gas identification among several one-nature gases.
{"title":"Investigation of Adsorption Kinetics on the Surface of a Copper-Containing Silicon–Carbon Gas Sensor: Gas Identification","authors":"Nina K. Plugotarenko, Sergey P. Novikov, Tatiana N. Myasoedova, Tatiana S. Mikhailova","doi":"10.3390/c9040104","DOIUrl":"https://doi.org/10.3390/c9040104","url":null,"abstract":"The low selectivity of materials to gases of a similar nature may limit their use as sensors. Knowledge of the adsorption kinetic characteristics of each gas on the surface of the material may enable the ability to identify them. In this work, copper-containing silicon–carbon films were formed using electrochemical deposition on the Al2O3 substrate with interdigitated Cr/Cu/Cr electrodes. These films showed good adsorption characteristics with several different gases. The adsorption kinetics of nitrogen dioxide, sulfur dioxide, and carbon monoxide on the film surface were investigated by the change in the resistivity of the material. Pseudo-first-order and pseudo-second-order kinetics, Elovich, Ritchie, and Webber intraparticle diffusion models were applied. It was found that the largest approximation factor and the lowest Root-Mean-Square Error and Mean Bias Error for all three gases were for the Elovich model. The advantages of silicon–carbon copper-containing films for gas sensor applications were shown. An algorithm for gas recognition was proposed based on the dependence of the change in the resistivity of the material under stepwise gas exposure. It was found that parameters such as the values of the extrema of the first and second derivatives of the R vs. t dependence during adsorption and the slope of R vs. t dependence in the Elovich coordinates are responsible for gas identification among several one-nature gases.","PeriodicalId":9397,"journal":{"name":"C","volume":"4 28","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135818228","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jorge S. S. Neto, Daniel K. K. Cavalcanti, Luiz E. da Cunha Ferro, Henrique F. M. de Queiroz, Ricardo A. A. Aguiar, Mariana D. Banea
The main objective of this research centered on investigating the effect of the addition of multi-walled carbon nanotubes (MWCNTs) on the mechanical and thermal properties of curauá-fiber-reinforced composites. The MWCNTs were added either to the fiber surface or into the resin matrix as the second reinforcing phase. The MWCNT-modified curauá fibers as well as raw fibers were characterized using a single-fiber tensile test, TGA, and FTIR analysis. Further, different composite samples, namely, pure curauá, (curauá + MWCNTs) + resin and curauá+ (resin + MWCNTs), were manufactured via compression molding and tested to determine their mechanical and thermal properties. Scanning electron microscopy (SEM) analysis was used to examine the surfaces of the tested fibers. It was found that the addition of MWCNTs to the curauá fibers resulted in positive effects (an enhancement in properties was found for the MWCNT-modified fibers and their composites). The addition of MWCNTs also increased the thermal stability of the natural fibers and composites.
{"title":"Effect of Multi-Walled Carbon Nanotubes on the Mechanical and Thermal Properties of Curauá Natural-Fiber-Reinforced Composites","authors":"Jorge S. S. Neto, Daniel K. K. Cavalcanti, Luiz E. da Cunha Ferro, Henrique F. M. de Queiroz, Ricardo A. A. Aguiar, Mariana D. Banea","doi":"10.3390/c9040102","DOIUrl":"https://doi.org/10.3390/c9040102","url":null,"abstract":"The main objective of this research centered on investigating the effect of the addition of multi-walled carbon nanotubes (MWCNTs) on the mechanical and thermal properties of curauá-fiber-reinforced composites. The MWCNTs were added either to the fiber surface or into the resin matrix as the second reinforcing phase. The MWCNT-modified curauá fibers as well as raw fibers were characterized using a single-fiber tensile test, TGA, and FTIR analysis. Further, different composite samples, namely, pure curauá, (curauá + MWCNTs) + resin and curauá+ (resin + MWCNTs), were manufactured via compression molding and tested to determine their mechanical and thermal properties. Scanning electron microscopy (SEM) analysis was used to examine the surfaces of the tested fibers. It was found that the addition of MWCNTs to the curauá fibers resulted in positive effects (an enhancement in properties was found for the MWCNT-modified fibers and their composites). The addition of MWCNTs also increased the thermal stability of the natural fibers and composites.","PeriodicalId":9397,"journal":{"name":"C","volume":"11 10","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135818219","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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